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Katrien Fret Mixtures Modeling of Steam Cracking of Complex Modeling of Steam Cracking of Complex Hydrocarbon Mixtures Katrien Fret Promotoren: prof. dr. Marie-Françoise Reyniers, prof. dr. ir. Guy Marin Begeleider: dr. ir. Kevin Van Geem Masterproef ingediend tot het behalen van de academische graad van Master in de ingenieurswetenschappen: chemische technologie Vakgroep Chemische proceskunde en technische chemie Voorzitter: prof. dr. ir. Guy Marin Faculteit Ingenieurswetenschappen Academiejaar 2008-2009 Modeling of Steam Cracking of Complex Hydrocarbon Mixtures Katrien Fret Promotoren: prof. dr. Marie-Françoise Reyniers, prof. dr. ir. Guy Marin Begeleider: dr. ir. Kevin Van Geem Masterproef ingediend tot het behalen van de academische graad van Master in de ingenieurswetenschappen: chemische technologie Vakgroep Chemische proceskunde en technische chemie Voorzitter: prof. dr. ir. Guy Marin Faculteit Ingenieurswetenschappen Academiejaar 2008-2009 VOORWOORD Deze masterproef was waarschijnlijk nooit uitgegroeid tot wat ze uiteindelijk is geworden zonder de hulp van een aantal mensen die ik hiervoor graag wil bedanken. Allereerst wil ik mijn promotoren, prof. dr. ir. Guy Marin en prof. dr. Marie-Françoise Reyniers, bedanken omdat zij mij de mogelijkheid hebben gegeven dit project uit te werken. Ik zou hen ook willen bedanken voor de opvolging van mijn werk en de belangstelling voor het onderwerp. Verder ben ik mijn begeleider, dr. ir. Kevin Van Geem, enorm dankbaar voor alle hulp en de grondige verbetering van mijn tekst. Zonder zijn kennis en inzet was ik niet in staat geweest om dit werk tot een goed einde te brengen. Bovendien wil ik Steven Pyl bedanken voor het beantwoorden van mijn vele vragen en al zijn hulp. Mijn dank gaat ook uit naar het technisch personeel, en in het bijzonder Michael Lottin, om voor alle problemen met de installaties een oplossing te bedenken en ook steeds klaar te staan bij moeilijkheden. Vervolgens wil ik al mijn medestudenten en iedereen van het LCT bedanken voor de leuke momenten tussen het werken door. In het bijzonder bedank ik Yuri, Michael, Wim en Sam voor de fijne momenten en ook om steeds een luisterend oor te zijn. Tenslotte wil ik ook mijn ouders en mijn twee zussen bedanken voor al hun steun gedurende de voorbije jaren en de kans die ik kreeg om in Gent te studeren en te wonen. Katrien Fret 1 juni 2009 FACULTEIT TOEGEPASTE WETENSCHAPPEN Vakgroep Chemische Proceskunde & Technische Chemie Laboratorium voor Chemische Technologie Directeur: Prof. Dr. Ir. Guy B. Marin Laboratorium voor Chemische Technologie Verklaring in verband met de toegankelijkheid van de scriptie Ondergetekende, Katrien Fret afgestudeerd aan de UGent in het academiejaar 2008-2009 en auteur van de scriptie met als titel: Modeling of Steam Cracking of Complex Hydrocarbon Mixtures verklaart hierbij: 1. dat hij/zij geopteerd heeft voor de hierna aangestipte mogelijkheid in verband met de consultatie van zijn/haar scriptie: de scriptie mag steeds ter beschikking gesteld worden van elke aanvrager de scriptie mag enkel ter beschikking gesteld worden met uitdrukkelijke, schriftelijke goedkeuring van de auteur de scriptie mag ter beschikking gesteld worden van een aanvrager na een wachttijd van…………jaar de scriptie mag nooit ter beschikking gesteld worden van een aanvrager 2. dat elke gebruiker te allen tijde gehouden is aan een correcte en volledige bronverwijzing Gent, 1 juni 2009 Krijgslaan 281 S5, B -9000 Gent (Belgium) tel. +32 (0)9 264 45 16 • fax +32 (0)9 264 49 99 • GSM +32 (0)475 83 91 11 e-mail: Petra.Vereecken@UGent http://www.lct.ugent.be/start/pages/1/en MODELING OF STEAM CRACKING OF COMPLEX HYDROCARBON MIXTURES Katrien Fret Promotoren: prof. dr. Marie-Françoise Reyniers, prof. dr. ir. Guy Marin Begeleider: dr. ir. Kevin Van Geem Masterproef ingediend tot het behalen van de academische graad van Master in de ingenieurswetenschappen: chemische technologie Vakgroep Chemische proceskunde en technische chemie Voorzitter: prof. dr. ir. Guy Marin Faculteit Ingenieurswetenschappen Universiteit Gent Academiejaar: 2008 – 2009 Abstract Currently there is an increasing tendency to use heavy hydrocarbon feedstocks such as light gas oils, vacuum gas oils (VGO) and kerosenes as steam cracker feed. Another trend is the growing use of butane as feedstock. For the simulation of steam cracking of certain hydrocarbon fractions, including heavy fractions, a few shortcomings exist in the simulation model developed at the LCT i.e. COILSIM1D. One of them is the small or nearly non- existing experimental database, which is used to verify the simulation results. Another insufficiency is the lack of complete characterization of the heavy feedstock. The solution to this problem is the new GCxGC at the LCT, which has a ‘time of flight’ mass spectrometer (Tof MS) and a flame ionization detector (FID). This GCxGC makes it possible to analyze the feed and the cracker effluent qualitatively and quantitatively. An extension of the experimental database is obtained by a pilot plant study of the cracking behavior of two C4 fractions, a bio-derived naphtha and two heavy condensates (Chapter 3). Both quantitative and qualitative GCxGC analyses of a FT naphtha, a petroleum naphtha and a kerosene fraction are performed to provide a complete characterization of these complex feedstocks (Chapter 2). These results will make it possible to create more detailed and accurate fundamental simulation models for complex hydrocarbon fractions. Finally, simulations are performed with COILSIM1D (Chapter 4). The steam cracking process is simulated under different experimental conditions for pure naphtha, pure ethane and mixtures of naphtha and ethane. Based on the limited set of simulation results it seems that improvements to the reaction network for steam cracking are still possible. Keywords: steam cracking, GCxGC, Fischer-Tropsch naphtha, kerosene, simulation Modeling of Steam Cracking of Complex Hydrocarbon Mixtures Katrien Fret Promoters: prof. dr. ir. G.B. Marin, prof. dr. M.F. Reyniers Coach: dr. ir. K.M. Van Geem Abstract: Currently there is an increasing tendency to several shortcomings exist in the simulation model use heavy hydrocarbon feedstocks such as light gas oils, developed at the “Laboratory for Chemical vacuum gas oils (VGO) and kerosenes as steam cracker Technology” (LCT) of Ghent University i.e. feed. Another trend is the growing use of butane as COILSIM1D (Van Geem, 2006). One of them is the feedstock. However, the experimental database for these small or nearly non-existing experimental database, fractions is limited or non-existing, making the simulation model for modeling this process, which is used to verify the simulation results. Another COILSIM1D, less accurate than desired. Therefore the insufficiency is the lack of complete characterization experimental database, which is used to verify the of the heavy feedstock. The solution to this problem is simulation results, is extended with results obtained from the new GCxGC at the LCT, which has a ‘time of cracking two C4 fractions, a bio-derived naphtha and flight’ mass spectrometer (Tof MS) and a flame two heavy condensates. Quantitative and qualitative ionization detector (FID). This GCxGC makes it GCxGC analyses allowed to determine the detailed possible to analyze the feed and the cracker effluent composition of the FT naphtha, a petroleum naphtha and qualitatively and quantitatively. a kerosene fraction. Extension of this methodology to Both an extension of the experimental database and other fractions and even other processes will make it possible to create more detailed and accurate GCxGC analyses are obtained during this master fundamental simulation models for complex thesis. This will make it possible to create more hydrocarbon fractions. detailed and accurate fundamental simulation models for complex hydrocarbon fractions. Keywords: steam cracking, GCxGC, naphtha, kerosene, C4 fraction, gas condensate, simulation II. COMPREHENSIVE TWO -DIMENSIONAL GAS CHROMATOGRAPHY OF STEAM CRACKING FEEDSTOCKS I. INTRODUCTION GCxGC is a recently developed chromatographic Steam cracking of hydrocarbons is one of the most separation technique which is based on separations in important processes of the petrochemical industry. In two distinctly different columns that are placed after this process hydrocarbons are cracked into each other. The 1 st dimension separation is based on commercially more important products such as light volatility, the 2 nd on polarity. One advantage of the olefins and aromatics. Feedstocks ranging from light combination of two independent separation alkanes such as ethane and propane up to complex mechanisms is that ordered structures for structurally mixtures such as naphthas and heavy gas oils are related components show up in the GCxGC converted at temperatures ranging from 500 to 900 °C chromatograms, see Figure 1. A detailed group type in tubular reactors suspended in large gas-fired separation is now possible. Between the two columns furnaces. Globally, naphtha is the most commonly an interface, a cryogenic modulator, is present. Its applied feedstock in crackers. main role is to trap adjacent fractions of the analyte A recent trend is the growing use of butane as eluting from the first-dimension column by cryogenic feedstock caused by the application of ethanol as cooling, and heating-up these cold spots rapidly to transportation fuel. In order to meet gasoline vapor pressure specifications, low boiling hydrocarbon components, such as butanes and even pentanes, must be reduced in ethanol/gasoline blends. An alternative
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